ARACMP),

48

Initial least-squares refinement of the ARACMP trial model made use of a data set collected with molybdenum radiation. Isotropic refinement of all non-hydrogen atoms converged at an R index of 0.13 using all data collected out to sin2 e/A ^{2 =} 0.35. A difference map calculated at this

juncture revealed the positions of all hydrogen atoms except for that one participating in the 0(10) ••• 0(10) hydrogen bond. Two half-hydrogen atoms were used to represent the hydrogen bonding scheme here, and anisotropic refinement commenced. Two cycles in which the coordinates and six- parameter temperature factors for each heavy atom were varied along with a scale factor reduced the R index to

0.097. No hydrogen atom parameters were refined. During this stage of refinement it became increasingly clear that the quality of the weaker and high-angle data was sufficiently poor to warrant recollecting the data set using copper

radiation. Experimental details for the collecting of this

second set of data have been given (see EXPERIMENTAL-

49

refined with the heavy atom temperature factors and a scale factor; a second matrix contained the coordinates for the heavy atoms. Difference maps calculated after each cycle of refinement failed to indicated anything but a disordered hydrogen-bonding scheme along the screw axis relating 0(10) to 0(10), and so this model was retained through subsequent refinements.

Once again enantiomorph determination was attempted.

Form factors for N and O were corrected as described

previously (49), as was the form factor for P (51), Structure factor calculations for both enantiomorphic sets of parameters were performed, and the results are shown in Table 14, The differences in statistical sums favor heavily the D- structure over the L-, As one might expect, the strength of this

indication is greater than that for the ARAU determination (Table 10), but not nearly as strong as for ARAC,HCl(Table 6), Although .of" for Pin CuKoc. radiation is nearly that of Cl-, the fact that the "neuter parameters" were used in the ARACMP determination and refined D- and L- parameters were used in the ARAC,HCl comparison would likely make the latter a more powerful test. And although the methods of enantiomorph determination for both the ARAU and ARACMP cases were

identical, the much larger Af" of P with respect to the ^A f"s

of N and o would make the ARACMP test more positive than the

ARAU test. The entire preceding discussion assumes of course

that in all cases the measured intensities are of equal

50

Table 14. ARACMP. 1tl2.Q Enantiomorph Determination

(L) (D)

R 0.062 0.057

Rw 0.01203 0.00993

GOF 2.47 2.25

(for M = 1859 data and s = 289 parameters) .

51

significance statistically. By Hamilton's R-ratio test(52), all three enantiomorph determinations are significant at the ^Ol = 0.005 level.

Continued refinement converged after 5 cycles with an R index of 0.046, a weighted R of 0.00665, and a goodness- of-fit of 1.69. All shifts were less than o.6~, save three . These three were for coordinate values associated with

0(2'), H0(8) and 0(8), which were oscillating about their means by approximately±~. Hydrogen atoms associated with 0(10) were dealt with in the following waya H(lO) was placed as accurately as possible from previous difference maps;

two half-hydrogens, H(10a) and H(10b), were placed 1/3 the distance along vectors from 0(10) to 0(10) atoms at

(½-x, 1-y, ½+z) and (½-x, 1-y, z-½). None of these hydrogen atoms were refined in the last several cycles. Final

parameters are listed in Tables 15 and 16. Observed and

calculated structure factors are in Table 17.

Table 15. Itmu ARACMP. 3H 2 0 Non-Hydrogen Atom Parameters and their Est mated Standard Deviations. The ~ and ¥.. coordinates have been multiplied by 105; all other parameters have been multiplied by 10 4 . The form of the a.ni.sotropic temperature factor is T = exp[-2/ (la* 2 Uu + ... +k.£b*c*U 23 )]. The final value of ~he extinction parameter g is (o.6~o.4)x 10- 6 e- 2 . X l. z Un - - U22 Uss U1.2 U1.3 U2s N(l) 3215(l6) 34607(16) 7937(6) 269(14) 270(14) 323 (18) 58 (14) -33 (13) ~48(15) C(2) 10348(21) 31695 (20) 7396 (9) 304(19) 311(19) 389(23) 54(18) -32(20) -26(19) 0(2) 16136(14) 33744(17) 8491(7) 311(14) 574(19) 704(24) 71(14) -148(16) -262(21) N(3) 10357(17) 26174(17) 54o4(7) 241(16) 351(19) 4o8 (23) 66(14) 12(16) -41(16) ~ C (4) 4l33(20) 23550(17) 4093 (8) . 319(17) 213(17) 309(21) 21(15) 30(19) 20(17) N(4) 4885(17) 18621(17) 2137(8) 299(17) 361(19) 481(23) 32(15) 13(19) -111(18) C(5) -3005 (20) 26549(20) 4832(10) 252 (19) 327(20) 486(27) 1(15) -19(19) -76(21) C (6) -3145 (20) 31970(19) 6711(9) 279(19) 292(19) 466(28) 41(16) 30(19) -50(20) p -24472( 5) 34556 ( 5) 8810(2) 202 ( 5) 270( 5) 186( 5) -6( 4) 12( 4) -16( 5) 0(5') -18626(14) 41016(14) 8144(5) 333(14) 343 (14) 280(15) -17(12) 30(11) -51 (12) 0(6) -24964(15) 30119(13) 6209(6) 402 (16) 366(14) 290(13) -61(13) 10(16) -40(13) 0(7) -31694(14) 37620(15) 9887(6) 280(14) 501(17) 426(17) -2 (12) -1(13) -120(16)

Table 15 (continued) 0(8) -20247(15) 29873(14) 11055(6) 393(17) 454(17) 321(16) 34 (13) 67(16) 61(16) C(l') 2848(20) 41043(19) 9821(8) 297(19) 309(19) 254(20) 35(15) -47(16) -16(18) O(l') -4260(14) 41129(12) 11156(6) 371(12) 282 (12) 277 (13) 43(11) 26(14) 39(13) C(2') 3560(21) 48357(19) 8247(8) 311(19) 305 (19) 281(23) -15(16) -54(17) -2 (17) 0(2 I) 7674(15) 47845 (15) 5736(6) 343(16) 457(17) 367(18) -10(13) 64 (14) 20(16) c (3') -4784(21) 50304(19) 7763 (8) 336(20) 277(19) 233(20) -17(16) -37(18) 28(16) 0(3 I) -5522 (14) 57879(14) 7327(7) 375(16) 305(14) 579(20) -12 (13) -100(16) 151(15) ~ c (4') -8460(21) 47706(19) 10418(7) 350(20) 240(19) 237(22) 41(15) 18(17) -29(17) C(5') -16831(21) 46096(20) 10365(8) 353(20) 324(22) 327(25) 20(17) 49(18) -64(19) 0(9) 31673(16) 34259(16) 4029(7) 525 (19) 424(19) 631(22) -2 (17) 48(20) -17(22) 0(10) 23258 (18) 46555 (18) 5033(8) 472(19) 616(20) 836(27) 19(16) 76(20) 24(22) 0(11) 39610(16) 37423(15) 9120(7) 464(19) 498(19) 500(24) -54(15) 37(20) -65 (20)

Table 16. Final ARACMP.JH20 Hydrogen Atom Parameters and Their Estimated Standard Deviations. Coordinate values have been multiplied by 103.

Atom _{~ Y.. z} B!A ^{2 ~}

HN(3) 147(2) 246(2) 490(11) 3.4(1.0) HN(4) 95(3) 168(3) 206(11) 5.4(1.3) H'N(4) 8(2) 165(2) 155 ( 9) 3.3(1.0) HC(5) -74(2) 249(2) 399(10) 2.8(0.9) HC( 6) -74(2) 343(2) 709( 9) 3.9(1.0) HC ( 1' ) 67(2) 405(2) 1110( 9) 2.4(0.8) HC( 2' ) 60(2) 521{2) 9 53 ( 8) 1.5(0.7) HO{ 2' ) 94(4) 499(4) 585(16) 10.7(2,3) HC( 3' ) -72 ( 2) 475{2) 645 ( 8) 0,9(0,7) HO( 3' ) -99(2) 586(3) 683(11) 4,3(1,1) HC(4') -75(2) 512(2) 1165( 8) 2.2(0,9) HC(5') -185(2) 435(2) 1212( 8) 2,5(0.9) H'C(5') -192(2) 505(2) 998(10) 3,9(1.1) H( 8) -225(3) 295(3) 1184(12) 4.4(1.5) H(9) 299(3) 305(3) 383(14) 603(1,5) H' ( 9) 281(4) 376(4) 440(18) 11.1(2.3) H(ll) 367 ( 3) 353(3) 1015(13) 5.2(1.5) H' ( 11) 376 (3) 379 ( 3) 779(14) 6,2(1,7) H{lO) 191{0) 451(0) 523{ 0) 12.0( 0)

H(lOa) 247(0) 488(0) 673( 0) 12.0( 0)

H( 10b) 247(0) 488(0) 339( 0) 12.0( 0)

55

Table 17. Observed and Calculated Structure Factors for

ARACMP.3H20• Each set of four columns contains, from left

to right, the h index, 10fF ₀ l, lOfFcl, and 10JF ₀ 2-Fc2 1/~(F ₀ 2 ).

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